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有机磷化合物的键离解能:对当代从头算程序的评估。

Bond dissociation energies of organophosphorus compounds: an assessment of contemporary ab initio procedures.

机构信息

Center for Molecular Modeling, Ghent University, Technologiepark 903, B-9052 Zwijnaarde, Belgium.

出版信息

J Phys Chem A. 2010 Mar 4;114(8):2864-73. doi: 10.1021/jp908502d.

Abstract

Thermodynamic properties of phosphorus-containing compounds were investigated using high-level ab initio computations. An extended set of contemporary density functional theory (DFT) procedures was assessed for their ability to accurately predict bond dissociation energies of a set of phosphoranyl radicals. The results of meta- and double-hybrids as well as more recent methods, in particular M05, M05-2X, M06, and M06-2X, were compared with benchmark G3(MP2)-RAD values. Standard heats of formation, entropies, and heat capacities of a set of ten organophosphorus compounds were determined and the low-cost BMK functional was found to provide results consistent with available experimental data. In addition, bond dissociation enthalpies (BDEs) were computed using the BMK, M05-2X, and SCS-ROMP2 procedure. The three methods give the same stability trend. The BDEs of the phosphorus(III) molecules were found to be lower than their phosphorus(V) counterparts. Overall, the following ordering is found: BDE(P-OPh) < BDE(P-CH(3)) < BDE(P-Ph) < BDE(P-OCH(3)).

摘要

使用高精度的从头算方法研究了含磷化合物的热力学性质。评估了一组当代密度泛函理论(DFT)程序,以确定它们预测一组膦基自由基键离解能的能力。比较了包括元杂化和双杂化以及较新方法(特别是 M05、M05-2X、M06 和 M06-2X)在内的结果与基准 G3(MP2)-RAD 值。确定了一组十种有机磷化合物的标准生成热、熵和热容,并发现低成本 BMK 函数提供的结果与可用的实验数据一致。此外,还使用 BMK、M05-2X 和 SCS-ROMP2 程序计算了键离解焓(BDE)。这三种方法给出了相同的稳定性趋势。发现磷(III)分子的 BDE 低于其磷(V)对应物。总的来说,发现以下顺序:BDE(P-OPh) < BDE(P-CH(3)) < BDE(P-Ph) < BDE(P-OCH(3))。

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